Abstract
Magnetism in van der Waals semiconductors offers significant potential for fundamental research on low-dimensional magnetism and the development of high-performance two-dimensional spintronic devices. Here, we report the growth, physical properties, and first-principles calculations of a new dual-octahedral transition metal chalcogenide (DTMC) MnSi2Te4. MnSi2Te4 features a layered structure with an intralayer heterostructure, where the metal octahedra and nonmetal dimeric octahedra form zigzag chains alternately. Property characterization reveals that MnSi2Te4 is a collinear G-type antiferromagnetic semiconductor, with a Néel temperature TN of 18.6 K and a significant unsaturated negative magnetoresistance (NMR) reaching −42.5% at 9 T and 100 K. First-principles calculations on the electronic band structure demonstrate that the large NMR primarily originates from the spin splitting due to parity-time symmetry breaking. This study not only discovers a new member of DTMCs with a unique crystal structure and large NMR, but also establishes a promising platform for investigating next-generation spintronic devices.
| Original language | English |
|---|---|
| Pages (from-to) | 340-348 |
| Number of pages | 9 |
| Journal | Journal of the American Chemical Society |
| Volume | 148 |
| Issue number | 1 |
| DOIs | |
| State | Published - Jan 14 2026 |
Funding
K.L. and G.W. would like to thank Prof. X. L. Chen of the Institute of Physics, Chinese Academy of Sciences, for fruitful discussions. B.Y. and Q.W. would like to thank Z. H. Liu and Z. Y. Song of the Institute of Physics, Chinese Academy of Sciences, for fruitful discussions. This work was partially supported by the National Natural Science Foundation of China (Grant Nos. 52325201 and 11888101), the National Key Research and Development Program of China (Grant Nos. 2023YFA1607400 and 2022YFA1403900), and the sample preselection and characterization station of the Synergetic Extreme Condition User Facility. We thank the staff from the BL07U beamline of the Shanghai Synchrotron Radiation Facility for their assistance with XAS data collection. The neutron part of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The beam time was allocated to the WAND instrument on proposal number IPTS-33282.1. This article has been authored by UT-Battelle, LLC under Contract DEAC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Attempts to synthesize DTMCs with a similar structure resulted in a layered nonmagnetic semiconductor MgSiTe, which features a similar intralayer zigzag arrangement but a different stacking order, suggesting the potential for further extending the DTMC family with a zigzag intralayer arrangement. 2 4 K.L. and G.W. would like to thank Prof. X. L. Chen of the Institute of Physics, Chinese Academy of Sciences, for fruitful discussions. B.Y. and Q.W. would like to thank Z. H. Liu and Z. Y. Song of the Institute of Physics, Chinese Academy of Sciences, for fruitful discussions. This work was partially supported by the National Natural Science Foundation of China (Grant Nos. 52325201 and 11888101), the National Key Research and Development Program of China (Grant Nos. 2023YFA1607400 and 2022YFA1403900), and the sample preselection and characterization station of the Synergetic Extreme Condition User Facility. We thank the staff from the BL07U beamline of the Shanghai Synchrotron Radiation Facility for their assistance with XAS data collection. The neutron part of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The beam time was allocated to the WAND2instrument on proposal number IPTS-33282.1.
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